CR Doped Cd3As2

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PHYSICAL REVIEW B 97, 085303 (2018)

Cr doping induced negative transverse magnetoresistance in Cd3 As2 thin films


Yanwen Liu,1,2 Rajarshi Tiwari,3 Awadhesh Narayan,3,4,5 Zhao Jin,6 Xiang Yuan,1,2 Cheng Zhang,1,2 Feng Chen,1,2 Liang Li,6
Zhengcai Xia,6 Stefano Sanvito,3,* Peng Zhou,8,† and Faxian Xiu1,2,7,‡
1
State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200433, China
2
Institute for Nanoelectronic Devices and Quantum Computing, Fudan University, Shanghai 200433, China
3
School of Physics, AMBER and CRANN Institute, Trinity College, Dublin 2, Ireland
4
Department of Physics, University of Illinois at Urbana-Champaign, Champaign, Illinois USA, 61801
5
Materials Theory, ETH Zurich, Wolfgang-Pauli-Strasse 27, CH 8093, Zurich, Switzerland
6
Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology, Wuhan 430074, China
7
Collaborative Innovation Center of Advanced Microstructures, Nanjing 210093, China
8
State Key Laboratory of ASIC and System, Department of Microelectronics, Fudan University, Shanghai 200433, China

(Received 17 August 2017; published 9 February 2018)

The magnetoresistance of a material conveys various dynamic information about charge and spin carriers,
inspiring both fundamental studies in physics and practical applications such as magnetic sensors, data storage,
and spintronic devices. Magnetic impurities play a crucial role in the magnetoresistance as they induce exotic
states of matter such as the quantum anomalous Hall effect in topological insulators and tunable ferromagnetic
phases in dilute magnetic semiconductors. However, magnetically doped topological Dirac semimetals are hitherto
lacking. Here, we report a systematic study of Cr-doped Cd3 As2 thin films grown by molecular-beam epitaxy. With
the Cr doping, Cd3 As2 thin films exhibit unexpected negative transverse magnetoresistance and strong quantum
oscillations, bearing a trivial Berry’s phase and an enhanced effective mass. More importantly, with ionic gating the
magnetoresistance of Cr-doped Cd3 As2 thin films can be drastically tuned from negative to positive, demonstrating
the strong correlation between electrons and the localized spins of the Cr impurities, which we interpret through
the formation of magnetic polarons. Such a negative magnetoresistance under perpendicular magnetic field and
its gate tunability have not been observed previously in the Dirac semimetal Cd3 As2 . The Cr-induced topological
phase transition and the formation of magnetic polarons in Cd3 As2 provide insights into the magnetic interaction
in Dirac semimetals as well as their potential applications in spintronics.

DOI: 10.1103/PhysRevB.97.085303

I. INTRODUCTION antilocalization (WAL) and weak localization (WL) [6,7].


More importantly, a quantum anomalous Hall effect has been
It is well known that magnetic doping can effectively
achieved by means of magnetic doping and proper Fermi-level
manipulate the magnetoresistance (MR) of a material and can
engineering [8–13].
possibly give rise to magnetism [1–4]. One notable example
At the same time, the great success of graphene and topo-
is that of dilute magnetic semiconductors, which combine
logical insulators [14–17] has generated a tremendous interest
in the same material the advantages of semiconductors and
in topologically protected semimetals. Hereinto, the existence
ferromagnets [1,3]. For instance, Mn substitution in GaAs
of Dirac semimetals, which host three-dimensional Dirac
provides a compound, (Ga,Mn)As, that exhibits negative MR
fermions in the bulk state, has been theoretically predicted
and carrier-mediated ferromagnetism, and several other mag-
and experimentally verified [18–22]. Among them, Cd3 As2
netically doped semiconductors and oxides have demonstrated
was identified to be an ideal Dirac semimetal, showing good
novel spintronic functionalities [3,4]. Another important ex-
chemical stability [21], extremely high mobility [22–24], and
ample is magnetically doped topological insulators (TIs). The
chiral anomaly induced negative MR [25–28]. The robust topo-
topologically nontrivial ferromagnetic phase and the magnetic
logical protection in Cd3 As2 has also been proved in different
quantum-phase transition to a paramagnetic trivial state have
geometries like bulk [22–24], mircobelts [25,29], nanowires
been, respectively, demonstrated in different TI systems when
[26–28], and thin films [30], making this material conveniently
increasing the magnetic doping [5]. The interplay between
exploited. When either the time-reversal symmetry or the
topological protection and the breaking of the time-reversal
inversion symmetry is broken, the degenerate Dirac nodes
symmetry by the magnetic impurity results in intricate MR
in a Dirac semimetal will separate into Weyl nodes, result-
behavior in TI thin films, such as the competition between weak
ing in a Weyl semimetal phase. While inversion-symmetry-
broken Weyl semimetals were realized in noncentrosymmetric
monosphides from the TaAs family [31–33], stable time-
*
Sanvitos@tcd.ie reversal symmetry-broken Weyl semimetals without coupling
† to orbital motion and spin through Landau quantization and
pengzhou@fudan.edu.cn

Faxian@fudan.edu.cn Zeeman splitting are still being sought. An external magnetic

2469-9950/2018/97(8)/085303(8) 085303-1 ©2018 American Physical Society


YANWEN LIU et al. PHYSICAL REVIEW B 97, 085303 (2018)

field or magnetic doping can implement the breaking of ESPRESSO code [39]. The rotationally invariant form of the
the time-reversal symmetry. A few theoretical studies have Hubbard U correction was used [40]. A plane-wave cutoff of
predicted a Ruderman-Kittel-Kasuya-Yosida interaction and a 545 eV was employed and the Brillouin zone was sampled
Kondo effect among the magnetic impurities in both Dirac and using an 8 × 8 × 4k-point grid for the self-consistent calcula-
Weyl semimetals [34–37], although the experimental evidence tions. The I41/acd space group with an 80-atom unit cell for
remains lacking. Cd3 As2 was used [41].
Here we report a systematic study of the magnetotransport
properties of Cd3 As2 thin films incorporating different con- III. RESULTS AND DISCUSSION
centrations of Cr doping. Our high-quality Cd3 As2 thin films
were grown by molecular-beam epitaxy (MBE), and a negative A. Growth and temperature-dependent resistance
transverse MR is observed in all magnetically doped samples, Cd3 As2 thin films were grown by MBE with different Cr
suggesting that the doping induces spin-dependent scattering doping concentrations. From our previous study we know that
from magnetic polarons. The evolution of the Shubnikov–de undoped Cd3 As2 thin films thinner than 50 nm will experience
Haas quantum oscillations indicates that the band structure and a band-gap opening and become trivial insulators [30,42].
the topological properties experience a topological quantum- Therefore, we primarily focus on Cd3 As2 thin films with a
phase transition from a nontrivial to a trivial phase, a phase thickness of about 100 nm, which is thick enough to hold
transition that is triggered by the Cr doping. Remarkably, the the Dirac feature. The Cr concentration can be fine-tuned by
MR can be electrically manipulated via ionic gating and the re- adjusting the Cr evaporation temperature during the growth
sulting switching between positive and negative MR serves as a (as discussed in the above experimental and computational
signature of magnetic polaron formation in Cr-doped Cd3 As2 . details). The composition of as-grown thin films is determined
These findings are in a good agreement with density-functional by energy-dispersive x-ray spectroscopy (EDX). It is found that
theory and Monte Carlo calculations. Our results represent Cr replaces Cd and yields the compound Crx Cd3−x As2 [43].
a step toward the manipulation of the topological Dirac The single crystallinity with the growth face of (112) plane
semimetal phase via magnetic doping, and pave the way for po- of the as-grown thin films is examined by x-ray diffraction
tential spintronic applications of topological Dirac semimetals. (XRD) [Fig. 1(a)]. Standard Hall bar devices were built from
the thin films. The temperature-dependent residual resistance
II. EXPERIMENTAL AND COMPUTATIONAL DETAILS R(T)/R(300 K) reveals the effect of the Cr doping. For undoped
thin films, the resistance increases as the temperature decreases
Cd3 As2 thin films were grown in a CREATEC molecular in the high-temperature regime and saturates at low tempera-
beam epitaxy (MBE) system with base pressure less than tures. As the Cr concentration increases, however, the samples
2 × 10−10 mbar. High-purity Cd (99.9999%), As (99.9999%), begin to exhibit a low-temperature metallic behavior, similar
and Cr (99.9999%) were evaporated by dual-filament, valve- to what was reported for half metals [44].
cracker, and single-filament effusion cells, respectively.
Freshly cleaved mica substrates were annealed at 350 °C
for 30 min to remove the molecule absorption. During the B. MR behavior of the Cr-doped Cd3 As2 thin films
growth process, the substrate temperature was kept at 225 To better understand the effect of the doping, we have per-
°C. The entire growth was in situ monitored by the reflection formed temperature-dependent MR measurements of different
high-energy electron diffraction system. The crystal structure Cr-doped Cd3 As2 thin films. The most striking feature arising
was determined by x-ray diffraction (Bruker D8 Discovery, from the Cr substitution is the doping induced negative MR.
Bruker Inc., Billerica, MA, USA). In order to reveal the intrinsic effect of the magnetic doping,
The thin films were patterned into standard Hall bar several representative samples are selected for the detailed
geometry manually. The solid electrolyte was produced as study (Fig. 2). The undoped sample exhibits several prominent
follows: LiClO4 (Sigma-Aldrich) and poly(ethylene oxide) features of MR behavior [Fig. 2(a)], distinct from the extremely
(Mw = 100 000, Sigma-Aldrich) powders were mixed with large MR ratio observed in the bulk counterpart [22,24].
anhydrous methanol (Alfa Aesar). The solution was stirred Around zero field, there is a small dip in the MR, ascribed
overnight at 60 °C and served as the electrolyte. After the to WAL, which is also observed in Cd3 As2 nanostructures
application of solid electrolyte, the device was kept at 350 K for [26–29]. Such MR behavior is reminiscent of the WAL in
30 min in vacuum to remove the moisture before the transport TIs and topological crystalline insulators [45,46]. According
measurements. to the recent theoretical predictions [47], the WAL in Dirac or
The magnetotransport measurements were performed in a Weyl semimetals originates from quantum interference, giving
Physical Property Measurement System by Quantum Design a positive MR near zero field. Such a WAL phenomenon has
with a magnetic field up to 9 T. A home-made measure- been observed in TaAs [32,48] and regarded as a transport
ment system including lock-in amplifiers (Stanford Research signature of Dirac and Weyl semimetals, apart from the chiral
830) and Agilent 2912 source meters was used to acquire anomaly [26,28,32,47–49]. With increasing the magnetic field,
experimental data. Pulsed magnetic-field measurements up to the positive MR caused by the classical cyclotron motion
60 T were performed at Wuhan National High Magnetic Field prevails over the quantum interference effect and the quantum
Center. oscillations are clearly identified. This suggests a high mobility
Density-functional-theory calculations were carried out by exceeding 2500 cm2 V−1 s−1 , a value that is consistent with
employing the Perdew-Burke-Ernzerhof form of the exchange- the measured Hall mobility of 2300 cm2 V−1 s−1 (Supplemental
correlation functional [38] as implemented in the QUANTUM Material, Fig. 2 [50]).

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FIG. 1. The temperature-dependent resistance of different Cr-doped Cd3 As2 thin films. (a) XRD spectra of as-grown thin films at different
doping concentration. (b) The temperature-dependent residual resistance of different samples. The heavily doped samples show metallic behavior
at low temperatures.

Just a tiny amount of Cr dopants (x < 0.05) suppresses In order to verify the negative MR, a high magnetic pulsed
dramatically the positive MR and provides a strong negative field up to 55 T was applied to different magnetically doped
contribution [Fig. 2(b)]. The fact that the WAL feature is still samples [Fig. 2(c)]. The lightly doped sample (x  0.1) shows
preserved at zero field strongly suggests that there is only a a negative MR below 10 T and then a largely suppressed
negligible change in the topology of Cd3 As2 at a light magnetic positive MR under higher magnetic field. The heavily doped
doping. However, the negative MR accompanied by the strong case, however, boosts the effect of the magnetic doping further.
quantum oscillations persists up to 9 T, implying another The heavily doped one (x  0.2) exhibits a negative MR up to
hidden mechanism rather than WL, which usually contributes ∼30 T with strong quantum oscillations. For magnetic fields
near zero field [47]. larger than 30 T, all the magnetically doped thin films display

FIG. 2. MR behavior of different Cr-doped Cd3 As2 thin films. (a), (b) The MR behavior at different temperatures for the undoped and
lightly doped samples with the same thickness of 100 nm. (c) The MR behavior of different doping samples under ultrahigh magnetic pulsed
field. (d) The thickness-dependent MR behavior for the heavily doped samples at 2 K.

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FIG. 3. Analysis of quantum oscillations. (a) The critical field and phase-coherence length of the lightly doped sample. (b) The critical
field and phase-coherence length of the different Cr doping samples at 2 K. (c) The Berry phase of the different doping samples, indicating the
quantum-phase transition from nontrivial to trivial state. The inset is doping-dependent oscillation frequencies. The error bars were generated
from the linear fitting process in the Landau fan diagrams. (d) The effective mass of different samples, suggesting that the Cr doping enhances
the effective mass. The quantum lifetime is extracted from the high-field quantum oscillations.

a rapidly growing positive MR, indicating that the system qi qi


Here the parameters C1 and C2 are positive for WL
approaches the quantum limit as all the carriers are condensed and negative for WAL, and the critical field Bc is related
into the lowest Landau level [51–53]. Such MR behavior in to the phase-coherence length φ according to Bc ∼ h̄/e2φ .
the quantum limit is confirmed by our following analysis of The phase-coherence length φ decreases from ∼150 to
the quantum oscillations and is consistent with what was also ∼60 nm with increasing Cr doping, directly suggesting the Cr-
reported in Cd3 As2 nanowires with low carrier density [26,27]. induced suppression of the WAL [Fig. 3(a)]. The temperature-
The thickness-dependent MR of heavily doped samples dependent φ of the lightly doped sample displays an abnormal
shows that the dimensionality serves as an additional factor evolution [Fig. 3(b)]. The φ saturates at low temperature,
influencing the magnetotransport. The MR of the thin films similar to the case of dilute fluorinated graphene, having
with a thickness of 50, 100, and 200 nm was measured, as spin-flip states induced by the local magnetic moment [54].
shown in Fig. 2(d). The negative MR ratio of the 50 nm
sample at 9 T is about 25%, while for the thicker samples
D. Quantum oscillations analysis
of 100 and 200 nm it is 10 and 2%, respectively. The thinner
sample gives a larger negative MR, showing that with reducing Quantum oscillations provide a wealth of information about
the dimensionality the transport charges have much stronger the band structure and the topological properties of materials.
interaction with the local magnetic moment [4]. The oscillation frequency SF is related to the area of the
Fermi surface and the Berry’s phase B is related to the
topological property, which can be extracted from Landau
C. Localization analysis fan diagrams according to the Lifshitz-Onsager quantization
In order to gain a quantitative understanding of the com- rule [55]: SBF = N + 21 − 2πB − δ = N + γ , where N is the
petition between WAL and the negative MR induced by the Landau level index, SF is obtained from the slope of the
Cr doping, we have extracted the phase-coherence length of Landau fan diagram, and γ is the intercept. Conductivity σxx
different Cr-doped Cd3 As2 thin films (Supplemental Material, is converted from ρxx and ρxy using σxx = ρxx /(ρxx 2
+ ρxy
2
).
Sec. 2 and Supplemental Material, Figs. 4 and 5), following Here, the integer indices N denote the σxx minima positions in
the formula for 3D Dirac or Weyl semimetals [49]: 1/B, while the half-integer indices represent the σxx maxima
√ positions. For Dirac fermions, the linear plot of 1/B vs N
qi B + B
2 2 2
qi B B intercepts the N axis at 0.5, which implies a nontrivial π
σxx = C1 2
qi
+ C2 c2 .
Bc + B 2 Bc + B 2 Berry’s phase, whereas a value of around zero represents a

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FIG. 4. Gate modulation of the magnetoresistance of the heavily doped sample. (a) The temperature-dependent resistance of different carrier
density. (b) The Fermi energy as a function of carrier density. (c) The MR behavior with different carrier density. (d) Density of states of the
undoped and Cr-doped samples (the Cr concentration is ∼4%).

trivial Berry’s phase [23,56,57]. The measured SF of different from the usual small mass in Dirac systems, reconfirming the
Cr-doped Cd3 As2 thin films increases from ∼17 to ∼37 T, topological phase transition.
suggesting the doping induced larger Fermi surface [Fig. 3(c)]. The carrier lifetime τ could be

obtained from the Dingle fac-
The intercepts provide evidence for a Berry phase transition tor RD ∼ e−D , where D = πm eBτ
. Because of the complicated
from nontrivial (the undoped sample) to trivial (the heavily MR background in small magnetic field, we have calculated
doped sample), unambiguously showing the topological phase the quantum lifetime from the high-field data of Fig. 2(f) for
transition [Fig. 3(c)]. better accuracy (Supplemental Material, Fig. 7). Uncharacter-
Such a quantum topological phase transition is also con- istically, the quantum lifetime becomes longer as we increase
firmed by the effective mass of charge carriers in the thin the Cr concentration. The quantum lifetime indicates the small-
films. Following the Lifshitz-Kosevich formula [55,58,59], the angle scattering that dephases the momentum eigenstates of
oscillation component Rxx could be described by the carriers and is sensitive to all processes related to the
Landau level broadening [22,23]. In fact, this could be directly
  witnessed from the much sharper quantum oscillations of
SF
Rx x ∝ RT RD cos 2π +γ , (1) the heavily doped samples than that of the undoped and
B
lightly doped ones. Scattering from the Cr impurities in turn
decreases the transport lifetime, which could be proved by
where RT and RD are the reduction factors accounting for the declining trend of the Hall mobility [Fig. 3(d)]. As Cr
the phase-smearing effects due to temperature and scattering, replaces the Cd ions, the spin-orbit interaction between Cd
respectively. The effective mass m∗ can be estimated from and As is significantly reduced, resulting in an increase of
the temperature-dependent oscillation Rxx according to the spin lifetime. Meanwhile, the local magnetic moment induced
2π 2 kB T m∗ /h̄eB
temperature-smearing factor RT ∝ sinh(2π 2 k T m∗ /h̄eB) , where
B
by the Cr impurities results in a series of well-resolved
kB is the Boltzmann’s constant, h̄ is the reduced Planck’s con- spin-polarized subbands under magnetic field [4], instead of
stant (Supplemental Material, Fig. 6). The resulting effective the degenerated Landau levels as in the undoped sample.
mass of carriers in different Cr-doped Cd3 As2 thin films can be As a result, the scattering is reduced by the alignment of
extracted [Fig. 3(d)]. It is clear that the effective mass increases spins through the external magnetic field, giving rise to the
from 0.03 me to 0.12 me with high Cr concentration. Such a enhanced quantum oscillations with relatively long quantum
heavy effective mass in the heavily doped samples deviates lifetime.

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YANWEN LIU et al. PHYSICAL REVIEW B 97, 085303 (2018)

E. Gate-tunable MR behavior the percolation threshold needed for long-range magnetism


In order to gain further insight into the mechanism leading to is reached only at a high Cr concentration [60]. We have
the negative MR by Cr doping, ionic gating has been applied to estimated that such percolation threshold is approximately at
the heavily doped thin films. Previously, gate-tunable quantum 10% (10% of the Cd sites are substituted with Cr) for a fourth-
oscillations and ambipolar effect have been demonstrated nearest-neighbor Cr-Cr exchange interaction, a concentration
in undoped Cd3 As2 thin films [42]. As the carrier density far beyond what is present in our samples. Furthermore, even
decreases, the resistance of the thin film increases, which is beyond the percolation threshold the critical temperature is
consistent with the electron-dominated transport [Fig. 4(a)]. driven by the long-distance exchange coupling, which we
The Fermi energy extracted from the quantum oscillations calculate to be small (see Supplemental Material, Table I). As
decreases from ∼100 to ∼20 meV, indicative of a good such, even in the case percolation is reached through a spinodal
tunability of the heavily doped thin films. Moreover, as the arrangement of the Cr ions [61] the expected TC remains low.
Fermi level moves toward the bottom of the conduction band, In brief, our theoretical analysis returns Cr-doped Cd3 As2 as
the MR turns from entirely negative to positive [Fig. 4(c)], a diluted paramagnet with a strong p-d coupling, namely it is
showing a similar behavior as that of the undoped sample similar to Mn-doped II-VI diluted semiconductors [62].
[Fig. 2(a)]. Consequently, the effect of Cr doping is weakened Monte Carlo simulations were applied to obtain the fer-
gradually when the carrier density decreases, or when the romagnetic transition temperature, TC , over the entire range
Fermi level moves away from the conduction band. This of Cr doping, where we use exchange parameters obtained
indicates that the Cr doping generates an effective impurity from our first-principles calculations. For all the four cases
band inside the conduction band. At low temperatures, the from the first to the fourth neighbor, the long-range order
Fermi level lies inside this impurity band and the negative is not generated until the Cr dopant reaches a percolation
MR plays the dominant role. When the Fermi level is shifted threshold at some critical concentrations of xc . Here, xc can
away from the conduction band by the ionic gating, it leaves reduce to 0.3 as one goes to a longer-range exchange including
this impurity band, leading to the suppression of the negative the fourth-neighbor exchange. As previously discussed, the
MR (Supplemental Material, Fig. 10). This model is also introduction of Cr dopants suppresses the WAL behavior
supported by our density functional theory calculations as and generates a mechanism giving rise to the negative MR.
shown in Fig. 4(d). For undoped Cd3 As2 , the projected density The interplay between quantum localization and the mag-
of states (DOS) shows a band gap of about 0.1 eV, which is netism is reminiscent of the magnetic polarons scenario in
bridged by the Dirac cone (not displayed here) as observed in diluted semimetals and oxides [4,63,64]. Magnetic polarons
the band structure. In contrast, in the heavily doped samples are formed by the interaction between the carrier spins with the
[see lower panel of Fig. 4(d)], a band emerges in the DOS localized spins of the magnetic impurities [4]. Our electronic
at the bottom of the conduction band, consistent with our structure calculations showing a significant spin split of the
experimental observations. Such a band originates from the p-d valence band support the hypothesis of the magnetic polarons
interaction between the Cr dopants and the valence band of the formation. Such polarons are likely to have a short polaron
native Cd3 As2 crystal, and there is a significant spin splitting of radius so that the percolation is not possible and no long-range
the bands. Such a mechanism is similar to other conventional ferromagnetic order is developed. Yet, the interaction between
diluted magnetic semiconductors, such as (Ga,Mn)As [4]. the transport electrons and the magnetic impurities remains
It is now fundamental to explore the mechanism behind strong and it can profoundly affect the transport properties.
the negative MR in our magnetically doped samples. From With the magnetic field, the spins between adjacent polarons
our experiments we find that the dopant concentration, the are aligned well along the field direction. Also, the random spin
film thickness, and the carrier density can all affect the of intermediate regions between magnetic polarons may be
amplitude of the negative MR. In conventional ferromagnetic aligned with the increasing magnetic field. As a result, the spin-
conductor, it is common to observe such negative MR due to dependent scattering by the magnetic polarons is suppressed,
the spin-dependent scattering [2]. However, in our samples, leading to a negative contribution to the magnetoresistance.
the ferromagnetism is not observed either in the transport Such a scenario can be also made plausible by several pieces
or the magnetization measurements, and the same picture is of evidence from our transport data. It has been demonstrated
confirmed by our Monte Carlo calculations (Supplemental that the magnetic polaron is favored by reducing the dimension-
Material, Figs. 4 and 9 and Supplemental Material, Sec. 3). ality of systems and by increasing the exchange constant and
According to the EDX analysis, the Cr impurities substitute carrier effective mass [4]. In our experiments with the thinner
for Cd in the Cd3 As2 . As a result, Cr impurities provide both samples the negative MR is more pronounced, whereas in the
local magnetic moments and hole doping. For the magnetism, heavily doped 400-nm-thick sample, which is the 3D case, the
the effective lattice is the Cd sublattice on which the localized negative MR is almost undetectable (Supplemental Material,
spins of Cr lie. However, intrinsic defects in the thin films Fig. 8 and Supplemental Material, Sec. 1). In thin films less
provide additional electron doping that compensates for the than 100 nm thick, however, the negative MR dominates the
holes originating from Cr. Long-range magnetism can then transport, suggesting the formation of magnetic polarons in
be potentially activated by the p-d coupling, which is indeed a quasi-2D case with the reducing thickness. All the heavily
strong as confirmed by our electronic structure analysis for doped thin films have a large effective mass exceeding 0.1 me .
Cr-doped crystals. However, the peculiar structure of the This is a fingerprint of the formation of magnetic polarons. The
Cd3 As2 lattice prevents the formation of a robust ferromagnetic second evidence is the carrier-density-dependent MR behavior
ground state. The Cd sublattice presents little coordination (see in the heavily doped sample. By decreasing the carrier density
detailed discussions in Supplemental Material, Sec. 4) so that through ionic gating, we observe the decrease of negative MR

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and finally a revival of the positive MR with the carrier density in 3D. In contrast, for the heavily doped samples the formation
of ∼2 × 1012 cm−2 . With low carrier density, the strength of of magnetic polarons is ascribed as the mechanism for the
interaction between the carriers and magnetic impurities is negative MR. Our results not only provide a direction on the
greatly suppressed, suppressing the magnetic polarons, similar research of Dirac semimetals, but also bring insights to the
to the gate-tunable ferromagnetism in the MnGe quantum dots potential spintronic applications based on topological Dirac
[65]. Consequently, quantum interference between electrons semimetals.
resumes the dominant role and the WAL emerges again.
ACKNOWLEDGMENTS
IV. CONCLUSION
This work was supported by the National Key Re-
In conclusion, we have systemically studied the transport search and Development Program of China (Grant No.
properties of Cr-doped Cd3 As2 thin films. Magnetotransport 2017YFA0303302) and National Natural Science Founda-
measurements were performed for the films with different tion of China (Grants No. 11474058 and No. 61674040).
doping level, thickness, and carrier density. The magnetic F.X. acknowledges the support from the open project of
doping induced metallic behavior and negative MR were Wuhan National High Magnetic Field Center (Grant No.
observed at low temperatures. From the analysis of quan- PHMFF2015003). A.N. acknowledges support from ETH
tum oscillations, we have demonstrated the doping induced Zurich. S.S. and R.T. acknowledge support from the European
topological quantum-phase transition from nontrivial Dirac Research Council (QUEST project) and from Science Foun-
semimetal to trivial dilute magnetic semimetal as the Cr doping dation Ireland (Grant No. 14/IA/2624). Part of the sample fab-
increases. For the lightly doped sample, the robust Dirac rication was performed at Fudan Nano-fabrication Laboratory.
feature is preserved, demonstrating that Cd3 As2 is a good Computational resources were provided by the Trinity Centre
platform to study the magnetic interaction of Dirac fermions for High Performance Computing (TCHPC).

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